Solar Energy Materials and Solar Cells, Vol.161, 162-169, 2017
Single-step sulfo-selenization method for achieving low open circuit voltage deficit with band gap front-graded Cu2ZnSn(S,Se)(4) thin films
In this study, we investigate the electrical, structural, and optical properties of band gap front-graded Cu2ZnSn(S,Se)(4) (CZTSSe) thin films grown by a modified single-step sulfo-selenization process from copper poor and zinc-rich precursor metallic stacks prepared by co-evaporation. To investigate how the bandgap was graded in connection with the compositional distribution, we calculated the bandgap energy distribution along the film thickness, based on the transmission electron microscopy and energy-dispersive X-ray spectroscopy composition profile. The band gap of the CZTSSe phase with high S content near the surface layer is determined to be 1.161 eV. From the surface to the bottom, there is a decrease in the S content of the CZTSSe phase, and the band gap subsequently decreases to, 1.029 eV, close to the value of CZTSe. From the results of dimpling-Raman and scanning transmission electron microscopy line scanning, we confirm that the S content drastically increases from the bottom to the top surface of the CZTSSe thin film. The CZTSSe thin-fihn solar cell exhibits a power conversion efficiency (PCE) of 10.33%, with an open-circuit voltage (V-oc) of 0.505 V, short-circuit current density (J(sc)) of 31.61 mA/cm(2), fill factor (FF) of 64.6%, and V-oc deficit of 525 mV. Compared with the performance of the CZTSe solar cell, which had PCE of 7.23%, Vac of 0.424 V, J(sc) of 32.83 mA cm(-2), FF of 51.9%, and V-oc deficit of 576 mV, the V-oc and Voc deficit of the CZTSSe cell improved considerably. The high Voc, low V-oc deficit, and less loss of J(sc) are attributed to the effect of band gap front-grading induced by S grading into the CZTSSe thin film.
Keywords:CZTSSe thin films;Sulfo-selenization;Band gap front-grading;Low open circuit voltage deficit